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Molecular Engineering of a Metal-Organic Polymer for Enhanced Electrochemical Nitrate-to-Ammonia Conversion and Zinc Nitrate Batteries

Angewandte Chemie - International Edition, ISSN: 1521-3773, Vol: 62, Issue: 48, Page: e202309930
2023
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City University of Hong Kong Reports Findings in Molecular Engineering (Molecular Engineering of a Metal-Organic Polymer for Enhanced Electrochemical Nitrate-to-Ammonia Conversion and Zinc Nitrate Batteries)

2023 OCT 27 (NewsRx) -- By a News Reporter-Staff News Editor at Daily Hong Kong Report -- New research on Engineering - Molecular Engineering is

Article Description

Metal–organic framework-based materials are promising single-site catalysts for electrocatalytic nitrate (NO) reduction to value-added ammonia (NH) on account of well-defined structures and functional tunability but still lack a molecular-level understanding for designing the high-efficient catalysts. Here, we proposed a molecular engineering strategy to enhance electrochemical NO-to-NH conversion by introducing the carbonyl groups into 1,2,4,5-tetraaminobenzene (BTA) based metal-organic polymer to precisely modulate the electronic state of metal centers. Due to the electron-withdrawing properties of the carbonyl group, metal centers can be converted to an electron-deficient state, fascinating the NO adsorption and promoting continuous hydrogenation reactions to produce NH. Compared to CuBTA with a low NO-to-NH conversion efficiency of 85.1 %, quinone group functionalization endows the resulting copper tetraminobenzoquinone (CuTABQ) distinguished performance with a much higher NH FE of 97.7 %. This molecular engineering strategy is also universal, as verified by the improved NO-to-NH conversion performance on different metal centers, including Co and Ni. Furthermore, the assembled rechargeable Zn−NO battery based on CuTABQ cathode can deliver a high power density of 12.3 mW cm. This work provides advanced insights into the rational design of metal complex catalysts through the molecular-level regulation for NO electroreduction to value-added NH.

Bibliographic Details

Zhang, Rong; Hong, Hu; Liu, Xinghui; Zhang, Shaoce; Li, Chuan; Cui, Huilin; Wang, Yanbo; Liu, Jiahua; Hou, Yue; Li, Pei; Huang, Zhaodong; Guo, Ying; Zhi, Chunyi

Wiley

Chemical Engineering; Chemistry

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